apae-memo-29, i
TRANSCRIPT
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' UNCLASSIFIED - 44 -TA r --·_ APAE-MEMO-29,
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* 'AUTHOR - R. D. ROBERTSON
-
CURRENT STATUS OF Afl'R-1 FUEL ELEMENT
METALLURGY
c photostat Price $. 3.30Microfilm Price $2• 4 0
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CONTRACT NO. AT(11=1)-318' Available from the. Office of Technical Services
Department of CommerceWashington 25, D. C.
ISSUED: JULY 230 1956
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CLASSIFICATION CANCELLEDli & li i //1D 28: F 882 DATE FEB 22 1957 441%
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For The Atomic Energy Commission: .: ': 1 6- (Ail
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DISCLAIMER
This report was prepared as an account of work sponsored by anagency of the United States Government. Neither the United StatesGovernment nor any agency Thereof, nor any of their employees,makes any warranty, express or implied, or assumes any legalliability or responsibility for the accuracy, completeness, orusefulness of any information, apparatus, product, or processdisclosed, or represents that its use would not infringe privatelyowned rights. Reference herein to any specific commercial product,process, or service by trade name, trademark, manufacturer, orotherwise does not necessarily constitute or imply its endorsement,recommendation, or favoring by the United States Government or anyagency thereof. The views and opinions of authors expressed hereindo not necessarily state or reflect those of the United StatesGovernment or any agency thereof.
DISCLAIMER
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fee r. iFUEL ELEMENT METALLURGY
The devolopment by ORNL of fuel elements for the APER-1 has been
based on the use of 304L as the cladding material with highly enriched
uranium dioxide and a small quantity of boron carbide dispersed in a
sintered matrix of stainless steel as the fuel bearing coree The baron
carbide is introduced into the matrix as a burnable poison for controlling
excess reactivity at start-up.
Powder metallurgy techniques are used in preparing the coreo
The core is clad by the use of roll bonding and the picture frame technique.
Finished cladding thickness is .005"o and finished core thickness is 00201 o
A metallurgical bond is obtained between core and cladding and between
cladding elements themselvese
The materials used in the fuel bearing core of plates for both
stationary and control rod fuel elements are:
Stainless Steel Powder - type 304 with high silicon in a
size less than 149 mic,·onso
T02 POwder = highly enriched grade containing approximately
88% uranium in which the U-235 isotope is upgraded to product
levelo The oxide is prepared by the reduction of hydrated oxide=
uranyl nitrates commonly cmlled the Geneva process. Particle
size is 44-88 micronsp and the oxide powder is free of
elinging fineso
B4C Powder - contains approximately 76% natural boron and is
screened to less than 44 micron sizeo
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The st,dnless steel, uranium dioxide and boron carbide powder
for each batch are weighed separately before blendingo The oxide powder
is weighed inside a special box arrangement for handling enriched material.
The three materials are introduced into a glass container and blended in
an oblique blendero A small amount of lauryl alcohol is added near the
end of blending,
The blended powder is transferred to the die cavity in a box-type
enclosure on a hydraulic press. The powder is cold campacted under a
pressure of 33 tons per square inche
Ten compacts are loaded in a stainless steel sintering boat which
is then introduced into a high temperature furnace and sintered for one hour
at 21000 Fo A dry hydrogen atmosphere with a dew point of at least =700 F
ia Tnmintained during sinteringo At the conclusion of the sintering opera-
tion, the compacts are visually inspected and reloaded in the original dieand coined to correct for the shrinkage which · occurs during sinteringo
Acceptable compacts are weighed and stored in a desiccator for subsequent
useo
The cladding for the core is originally composed of three parts,
the frame for enclosing the four lateral edges Jf the zintered compact and
a top and bottom cover shield0 The frame piece is prepared by punching a
nearly square hole in plate material. The previously prepared core is
inserted in this hole in the frame and the cover pieces placed over and under
and welded to the frawe to form a three ply billeto
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The jacketed compact or billet is preheated before rolling to a
temperature of 21000 F for approximately 20 minutes in a muffle furnace
purged with hydrogeno The compacts are hot reduced on a 201' diameter and
301' face mi31 from 0390" to 00408 with a total reduction of approximately
90%0 The jacketed compacts are reheated for a minimum 0*,23minutes between
each pass xna after the final passo 'Hot reductions per pass are from 10
to 30%e Rolling direction is reversed after each passo After hot rolling
the scale is removed by pickling in an acid bath, and wire brushingo
The hot rolled plates are fluorcscoped to locate the outlines of
the core and the plate is marked for shearing. The fluoroscope examination
is also used as an inspection for gross segregation. The edges of the
composite plates are then trimmed to remove excess material and squared byshearingo
The plates are then cold rolled to a finished thickness of .030"°A 4 high mill with a 51' diameter work roll and 141' face is used. The re-
duction per pass is kept to less than 5% with total cold reduction approx-
imately 25%. The roll faces are lubricated with oil which is removed from
the finished plate by vapor degreasingo
The plates as cold rolled are wavy and archedo A flattening anneal
is required to bring the plates to acceptable flatnesso The plates are
batch stacked, pressure is applied between two bolt down platens with
aluinins being used to prevent sticking during annealingo Annealing is
done in an atmosphere of dry hydrogen at 2100' F for approximately two hours
followed by furnace cooling.
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. .The fuel plates are then refluoroscoped to locate the boundaries
of the core sectiono The core is positioned within dimensional limits speci-
fled in drawings D9=13=2007, D9=13-2006, A9=13-2010 and A9-13=20(1& 9 by means of
a template placed over the fuel plate. The outline of the finished fuel plate
ts marked for removal of excess inactive stainless steelo Finished specified
fuel plate size is obtained by shearing and batch machining to drawings I
89-13-20068 2007, A9=13-2010 and A943=2009. Machining lubricants are removed
by vapor degreasingo
Side plates with longltudinal grooves ninning the length of the plate
are gang milled to drawings D9-13-20119 2014, to provide the recesses for the. side edges of the fuel plates. Combs are also machined, primarily for use as
supports for the ends of the assembled plates during the brazing operationo
The 18 fuel plates (16 in the ease of control rod elements), 2 side
plates and 2 combs are assembled for brazing. Coast Metals NP brazing alloy,
containing 50 Nip 27=Fe, 11-St, 8-Mo, 4=P nominally, is usedo A stainless
steel brazing jig supports the assembly in loading and brasing. A pair of side
plates and one end comb are initially positioned in the jigo The first fuel
plate is then introduced into positiono The jig is rotated in two directions
to 45' from the horizontal so that brazing alloy powder can be loaded in the
flat position and eemented with Nicro-braze eement. A special technique is
used to insure the location of the brazing alloy to prevent excessive spreading
anto the fuel plate during brazingo This procedure ls repeated for each plate
Until All plates have been assembledo
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-dwill.ili;-The stainless steel brazing jig with the fuel element loaded is then
put into a muffle type brazing furnace. Helium is used as a purging gas at
low temperatures and pure dry hydrogen at high temperatureso Brazing tempera-ture is 2150* F and the unit is held at temperature for 5 minutes. Cooling
rate is governed by allowable distortion. Hydrogen is replaced by helium at a
temperature of approximately 1400' Fo
Fuel plate location and flatness are held to plus or minus 10% of
plate spacing except for the two outside plates. Tolerance on these plates as
measured down from side plate edges is plus or minus 5%.
End adapters are then welded to the ends of the stationary elements
after facing the endso The assembly is then machined to final dimensions per
drawing R943-1003. On the control rod fuel elements, a handle is welded to
the top end of the side plate before assembly and brazing. After brazing, a
pin is inserted through and welded to the handleso Assembly is per drawing
89=13-1004. The fuel element assembly is checked for squareness and lengthwisebowing by insertion in a box in which the inside dimensions are approximately
000310 amr the nominal fuel element external dimensionso
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fl.....8SPECIFICATIONS
Specifications for the manufacture of fuel elements and absorber
sections are being prepared in cooperation with Oak Ridge National Laboratory
personnel and are presently in final revisiono Fuel element loadings are as
follows:
Stationary Fuel Elements - per element
Fuel content - gro U-235 515o16+o38%
Enrichment = Product level lool%
Boron 10 - gro Oo483 +1075%
4.94%
Control Red Fuel Elements - per element
Fuel content - gre U-235 417*76+o38%eo59%
Enrichment i001%
Boron 10 = gro 00392 +1675%94094%
Tolerances are determined by aecuracies obtainable in analysiso weighing
and handlingo
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h.11'193111'91
FUEL ELEMENT IRRADIATION TESTS
Three test programs were undertaken to investigate the ability of
APPR-1 type fuel elements to perform satisfactorily.
One of these test4 described in detail in CF 5594-164 consisted of
exposure of encapsulated small sized specimens in the MTR. Test variations
in these samples included type of matrix material, type of oxide, initial oxide
particle size, oxide and poison contentsp burn=up and clad=core=clad proper=
tionso Examination of eight of these small sized samples has been made to date
by the Solid States Division of ORNLo Five of these samples received approxi-
mately 20% burn=up and the other three approximately 50% burn-upo On all
* eight samples no cracksp distortion, blistering, or other observable defects
were observedo
1.
Considerable effect of oxide particle size on hardness and ductility
of the stainless matrix material has been foundo On the 20% burn-up samples,
bend tests show fairly extensive core break=up in the oxide particle size range
of 7 to 11 microns. Minute core cracking was observed with oxide particle size
of 31 to 44 microns, 53 to 62 micron particles showed no evidence of cracking on
bendingo In general, samples containing oxide sizes under 31 microns showed
fairly extensive break-up while samples with larger particle size showed only
minute cracking in the range of 31 - 44 micronsp and no cracking with larger.
sizes. On the samples with 50% burn-upp there is not yet enough evidence to
establish a pattern. Complete evaluation must await examination of all -
irradiated sampleso
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00==IrHardness measurements also indicate the effect of oxide particle
size on hardness of matrix material under irradiationg as illustrated inthe following table:
HardnessOxide Particle Size VIIP = 2 KG Lead
(Microns) Before Irradiation 8fter Erradiation
7-11 204 475
31-44 184 42o
88 " 105 178 371
Although these results are not strictly conclusive because of the
limited number examined, the data indicates that particle sizes under 31 microns
have considerably more radiation-damage effect upon the matrix material thanlarger particle slzeso
Another irradiation testy described in detail in CF 55-6-39, consistedof exposure in the MTR 02 a full sized fuel elemenit adapted to MTR size require-ments. This full sized element received an estimated burn-up of 25 to 40%.Telescopic eicamination of the element as a unit, and of four plates removedfrom the elements showed.no defects except a possible crack in a small section
of a brazed jointo Metallurgical examination of the section containing this
questionable area revealed a surface irregularity rather than a cracko A
reddish-brown film ouilining the core section was evident cn all fuel plates.The third irradiation test, described in GF 5441-13 and CP 554-113,
was of a full sized element in the STR core at ARCOo However, this element hasreceived only a small portion of its proposed burn=up at the time of its removal
from the core some time agoo Corrosion resistance under STR operating conditions
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e.'1-ilizMhas been reported as excellento
In brief, all APPR-1 irradiation tests to date indicate that satis-
factory performance can be expected from APPR-1 fuel elements.
..
CONTROL RODS
It is presently planned to use Boron 10 as the absorber material in
the APPR control rods, dispersed in an iron matrix and clad with 304L stainless
steelo The method of fabrication is in general similar to that used in the
fabrication of the fuel bearing plates, with some variations due to the
difference in materials and end requirementso The picture frame technique is
again used as are powder metallurgy techniques for the preparation of the
Boron 10 and iron compacto Finished thiclcness of the absorber plate is .187"
' including 0032" claddingo Four plates are welded by the heliarc method into a
hollow box which is used in order to take advantage of the thermalizing effect
of the water in the center of the box on any fast neutrons which pass through
the sides of the box. Pertinent drawings are 89-13-2017 and 1002.
Absorber section loading is as follows:
Per element+
Boron 10 - gro 56o4 = 2% (tentative)
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tior:Immilum:'ll"/4ABSORBER IRRADIATION TESTS
The absorber plates were originally specified in ORNL-1613 as
dispersions of B in a copper matrix ana clad with 304L stainless steelo
Development work at ORNL on absorber plates was continued on this ccmbina-
tion of materials. It soon became evident, however, that copper cored stain-
less clad plates could not be fabricated satisfactorily due to the differences
in properties of copper and stainless steel at hot rolling temperatures. A
wide range of temperatures was trieds but in all cases it appeared that copper
was flowing between the stainless ftame elements themselves, resulting in poorbondingo Welding of frame elements of the plates was considered, but wasrejected because it was doubtful that a good seal could be obtained
consistentlyo
A review of potential absorber and matrix materials was then instituted.
Other compounds of boron were unattractive because of the larger weight percent
amounts *hat would be required due to the smaller weight percent of boron in
these compoundso Stainless steel, nickel, and nickel alloys had to be eliminated
as matrix materials because of evidence of reaction with the boron compounds
occurring at hot rolling temperatures. Boron 10 appeared to be a desirable
absorbing element because of the much smaller amount of total poison required I
per absorber plateo At this timep however$ boron 10 was apparently in rather
short supply and obtainable from only one source. Further investigation revealed
that boron 10 in the quantities required for APPR-1 could be obtained from
ORNLo
Development work was therefore initiated on using boron 10 as the
absorber and iron powder as a matrix material. It was found that rolling could
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-Ii/:.be performed in only one direction due to necessity for maintaining a square
and full thickness of core at the end adjacent to the fuel element. Also, since
starting thickness ef frame and covers is limited by ORNL press eapacityp
finished absorber plate thickness has been reduced to .187:' in order So obtain
the reduction desired for satisfactory bonding. This devel@pment work has
resulted in an absorber plate which is considered excellent from the structural
viewpointo
Considerable coneern, however, has developed as to the capability of I
beram=containing control rads to withstand irradiationo Under irradiation boron
is transibmmed into Lithium 7 and hellumo Calculations by ORNL personnel indicate
that the helium pressure resulting from bcron burn-up gould be·excessive pro=
vided the helium atoms formed diffused into a vcido Unfortunately, there is no
irradiation experience direetly comparable to the boron 10 dlsperston in aniron matrix proposed for the AI Pit=lo Wrought stainless steels containing boron
in amounts less than that required for APPR-1 absorber plates beeame tremendously
embrittled under irradiationo Blisters or warts have developed #m an wmelad
irradiated 1% boron dispersion in titaniume Cracks have developed under trradia=
tien in an unclad dispersion of boron in zirconiumo Howeverp due to differences
in properties of materials, and of the finished plates, there.is a very good
possibility that the boron 10 dispersions in irma clad with .032¤ of stainless
steel will not develop irregularities or defgats which would bar them from giving
satisfactory serviceo The clearance between the control red housing and the
absorber box section is sufficiently large that a gross dist6rtion or a gross
surface blistering would be necessary to cause interferenee with the proper
funetirning of the control rod assemb»o
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Im order to attain irradiation damage experience as soon as possibleD
a program has been set up to make and irradiate small samples of boran dispersed
in iron and clad.with stainless steel. These. small samples will be inserted
in leaky rabbits and irradiated in the MTR in a manner similar to the Phase XI
APER-1 fuel element samplese The proposed test samples and irradiation cycles
are listed in the table below4
Tee Emijazg/1 ErloriSE
B Design Loading 1 110 2 S3 34 45. 5
. 460% Bgo Dasign loading 3 6
5 7
12% 810 D"ign Loading 3 85 9
Low Deasification Core * 3 10
High m . 0 3 11
Low m " * 5 12High n w 0 5 ·3 3
*These samples have subsequently been eliminated from the test.programo
This test is based upon the assumption that five MTR cycles are the
equivalmnt of 100% burn=up and that five.cycles will require appradmately 15
weeks irradiation. The 60% B content samples are included because preliminary10
calculations indicate that this content will furnish the required blackness at
the end of one eore lifee Xt isp of coursep necessary to check this content in
a....."Up1 K, C 013
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./0."=the APPR-1 low power tests at Schenectady. The sample containing 20% excess
B is included as a possible accelerated teste The low and high densificatian10
samples are included to determine the effects of processing variableso
These thirteen samples are presently being fabricated and it is ex=
peeted that they will be shipped to the MTR by June lsto Xt is also planned
to test a full size control rod adapted for insertion in the MTRo This full
sized element ls in the stage of prellminary design at the present timeD and itis expected that it will be fabricated and shipped to the MTR in ally.
. Xh the event that these tests prove 40 to be an unS esirable absorber
material, consideration has been given to other materials for both immediate
and long range baek-up effetso Calculations have been made by Alco which
indicate that Hafnium would be a satisfactory substitute absorber materiale
I*
A hollow box constructed of solid Hafnium with walls .3" «i .4' thick is required.
'. 1The awmilability of Hafnium for this purpose is being investigated by ARBo0
Practically all potential absorber materials have been considered by
Alco personnel and evaluated.in connection with the long range back«up efforbo
High cross section rare earth materials appear unsatisfactory with present fab=
rication teclmiques because of the large,amount of eaeh material that would be
required to attal[n readivity control throughout core life equivalent to the
present design using 8100 St is entirely possible, of course, that a new fabrics=
tien teelmique can be developed which would permit the inearporation of the
relatively large amount of materials neededo Cadmium, Possibly in the form of
a eadmilm silver alloy at a content of about 30%, appears to be a more likelylong range back=up material at this timeo Wall thicknesses again in the crdew
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of .041, would be requ:isedo An experimenfnl reactivity evaluation of any alternate
absorber material in the APPR-1 core is required before a final decision can be
made to use a material other than borono
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